Simultaneous photocatalytic hydrogen production and CO2 reduction (to form CO and CH4) from water using methanol as a hole scavenger were investigated using silver-modified TiO2 (Ag/TiO2) nanocomposite catalysts. A simple ultrasonic spray pyrolysis (SP) method was used to prepare mesoporous Ag/TiO2 composite particles using TiO2 (P25) and AgNO3 as the precursors. The material properties and photocatalytic activities were compared with those prepared by a conventional wet-impregnation (WI) method. It was found that the samples prepared by the SP method had a larger specific surface area and a better dispersion of Ag nanoparticles on TiO2 than those prepared by the WI method, and as a result, the SP samples showed much higher photocatalytic activities toward H-2 production and CO2 reduction. The optimal Ag concentration on TiO2 was found to be 2 wt%. The H-2 production rate of the 2% Ag/TiO2 SP sample exhibited a six-fold enhancement compared with the 2% Ag/TiO2 WI sample and a sixty-fold enhancement compared with bare TiO2. The molar ratio of H-2 and CO in the final products can be tuned in the range from 2 to 10 by varying the reaction gas composition, suggesting a viable way of producing syngas (a mixture of H-2 and CO) from CO2 and water using the prepared Ag/TiO2 catalysts with energy input from the sun. Copyright (C) 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.